Single-crystal diamond (SCD) in particular in form of thin membranes [1][2][3] has gained an ever-increasing scientific interest over the years based on diamond's exceptional optical [4,5] and electrical [6,7] properties. Therefore, it has emerged as a highly promising platform e.g., in the field of nanophotonics for photonic integrated devices [8][9][10] and envisioned applications in quantum information technologies (QITs), such as quantum memories [11,12] and quantum communication. [13,14] Different kinds of optically active point defects in the SCD lattice, the so-called color centers like the nitrogen-vacancy (NV) center [15,16] or the silicon-vacancy (SiV) center, [17,18] show favorable characteristics, e.g., high photostability at room temperature and practicable control of coherent single spins, to serve as single-photon emitters in QITs.However, due to the high refractive index of diamond (n d % 2.41) [19] inducing total internal reflection at the diamond-air interface, light-confining architectures like nanopillars, [20,21] solid immersion lenses, [22,23] photonic crystal cavities [24,25] or Fabry-Pérot microcavities [26] are necessary to yield an efficient outcoupling from the zero-phonon line (ZPL) of the color centers and to improve the photon collection efficiency. For a strong and selective Purcell enhancement of the ZPL, cavities with a small mode volume and high-quality factor are required. One promising approach is the introduction of thin diamond membranes in fiber-based microcavities. [3,27] While such microcavities allow for spatial and spectral tunability as well as a direct outcoupling of photons in a single-mode fiber, the system efficiency can be limited by additional losses introduced by the diamond itself. Here the most crucial parameter is the surface roughness of the SCD membrane leading to scattering at the diamond-air interface. [28,29] For an effective Purcell enhancement and to maintain a high finesse, the membrane should be a few micrometers thick only, and the root mean square (rms) roughness should be as low as possible (minimum < 0.5 nm over the area of the cavity beam waist). [30] To achieve the desired long optical and spin coherence times for QIT applications, the membrane needs to be virtually free from lattice defects, paramagnetic impurities, and charge traps. This requires an initial removal of the damaged surface layers of the cut and polished starting material. [31] To reach